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Host (CdS)-guest (single-atomic Au) electron transfer mechanism for blue-LED-induced atom transfer radical addition of alkenes
Journal of Catalysis ( IF 6.5 ) Pub Date : 2022-06-03 , DOI: 10.1016/j.jcat.2022.05.016
Xiao-li Hao , Xiao-shan Chu , Ke-ling Luo , Wei Li

Atom transfer radical addition (ATRA) is commonly applied to introduce perfluoroalkyl groups into organic molecules, but it often suffers from harsh reaction condition, poor yield and expensive catalyst usage for practical application. Light-induced ATRA reaction is of great significance due to its merits of mild reaction condition and easy operation, but it is generally difficult to achieve high yield because of the lack of ideal photosensitizers. Herein, an Au single-atom sites (SASs) decorated hexagonal cadmium sulfide (CdS) nanocatalyst (CatCdS-Au) was synthesized to catalyze ATRA reaction under mild blue-LED-induction. As a result, the synergetic effect of CdS-Au interaction enhanced the optical properties and promoted the host (CdS)-guest (Au) electron transfer, leading to high ATRA yields (88–98%) and excellent selectivity even choosing different alkene substrates, which is remarkably superior over existing reaction systems (60–90% yields) ever reported in literatures. The present work sheds light on realizing high ATRA reaction yield via a green and high-efficient synthetic strategy.



中文翻译:

用于蓝色LED诱导烯烃原子转移自由基加成的主体(CdS)-客体(单原子Au)电子转移机制

原子转移自由基加成法(ATRA)通常用于将全氟烷基引入有机分子中,但在实际应用中往往存在反应条件苛刻、收率低和催化剂使用昂贵等问题。光诱导ATRA反应具有反应条件温和、操作简单等优点,具有重要意义,但由于缺乏理想的光敏剂,一般难以获得高产率。在此,Au 单原子位点 (SAS) 修饰了六方硫化镉 (CdS) 纳米催化剂 (Cat CdS-Au) 被合成以在温和的蓝色 LED 诱导下催化 ATRA 反应。因此,CdS-Au 相互作用的协同效应增强了光学性质并促进了主体 (CdS) - 客体 (Au) 电子转移,即使选择不同的烯烃底物,ATRA 产率也很高(88-98%)和优异的选择性,这明显优于文献中报道的现有反应系统(60-90%产率)。目前的工作为通过绿色高效合成策略实现高 ATRA 反应产率提供了启示。

更新日期:2022-06-06
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